Many materials offering high surface areas and/or advantageous chemical or electrical functionality are not widely utilized because they are difficult to handle and/or are not convenient to manufacture into usable forms. For example, with their remarkably high theoretical surface areas (14,600 m2/g) and vast potential for structural tunability, metal-organic frameworks (MOF) and their functionalized analogues can exhibit truly unique adsorption properties for gas/vapor systems, including high capacities and tailored selectivity. Applications can include toxic gas storage/separation, chemical sensing, catalysis, energy storage, heating and cooling, water management, efficient contrast imaging agents (acoustic, MRI etc.) and targeted extraction of critical metals from geothermal brines. However, conventional synthesis strategies for MOFs generally result in the formation of either dry powder products, with exceptionally low density, or colloidal suspensions. These inconvenient forms have limited their use to niche application spaces. More widespread industrial use of MOFs will continue to be limited given the poor mechanical strength and the difficulties faced with handling and processing these powders into useable form factors. Attempts to address the challenge have typically compromised the advantageous material properties that make MOFs attractive. Accordingly, there is an explicit and growing need for feedstock compositions and methods of making same that enable the production of engineered forms of MOF-based materials so that 3D objects of any desired shape or geometry can be realized.